Smits appeared as Senator Bail Organa of Alderaan in Star Wars: Episode II – Attack of the Clones (2002) and Star Wars: Episode III – Revenge of the Sith (2005), in which the character becomes Princess Leia's adoptive father. He reappeared as Bail Organa in the game Star Wars: The Force Unleashed (2008) and in the upcoming Rogue One: A Star Wars Story (2016).

In the third season of Dexter (2008), Smits played the murderous District Attorney Miguel Prado, one of the chief antagonists of the season along with Jesse Borrego's character. Smits was nominated for an Primetime Emmy Award for Outstanding Actor in a Drama Series for the role.